Sustainable zinc-air batteries (ZABs) are considered promising energy storage devices owing to their inherent safety, high energy density, wide operating temperature window, environmental friendliness, etc., showing great prospect for future large-scale applications. Thus, tremendous efforts have been devoted to addressing the critical challenges associated with sustainable ZABs, aiming to significantly improve their energy efficiency and prolong their operation lifespan. The growing interest in sustainable ZABs requires in-depth research on oxygen electrocatalysts, electrolytes, and Zn anodes, which have not been systematically reviewed to date. In this review, the fundamentals of ZABs, oxygen electrocatalysts for air cathodes, physicochemical properties of ZAB electrolytes, and issues and strategies for the stabilization of Zn anodes are systematically summarized from the perspective of fundamental characteristics and design principles. Meanwhile, significant advances in the in situ/operando characterization of ZABs are highlighted to provide insights into the reaction mechanism and dynamic evolution of the electrolyte|electrode interface. Finally, several critical thoughts and perspectives are provided regarding the challenges and opportunities for sustainable ZABs. Therefore, this review provides a thorough understanding of the advanced sustainable ZAB chemistry, hoping that this timely and comprehensive review can shed light on the upcoming research horizons of this prosperous area. 

Sustainable zinc-air battery chemistry: advances, challenges and prospects.

Stable operation of sustainable Zn–air batteries (ZABs) has attracted considerable attention, but it remains a huge challenge to achieve temperature‐adaptive and fast‐charging ZABs. The poor Zn|electrolyte interface and the sluggish charging kinetic are the major obstacles. Here, high‐performance ZABs are constructed by designing polarized zincophilic solid‐state electrolyte (SSE) with the unique solvation interaction of Zn2+ with ethylene glycol (EG), and atomic Mo site cathode catalyst. On the one hand, the modulation of the solvation structure of Zn2+ ions by partial substitution of H2O with EG inhibits Zn dendrite growth and parasitic reactions, leading to the improvement of the Zn|electrolyte interface. Moreover, the polarized terminal groups in SSE are strongly coordinated with Zn/H2O, which exerts a profound influence on Zn|electrolyte interface stability and low‐temperature properties. On the other hand, atomic Mo incorporated α‐Co(OH)2 mesoporous nanosheets decrease the overpotential of oxygen evolution reaction via strong electronic interaction. Consequently, the assembled aqueous ZABs exhibit ten‐time fast‐charging ability and remarkable cycling stability. Moreover, the assembled solid‐state ZABs show unprecedented stability (1400 cycles at 5 mA cm−2) and high energy efficiency at −40 °C.

Electrolyte Tuned Robust Interface toward Fast‐Charging Zn–Air Battery with Atomic Mo Site Catalyst

The low energy efficiency and limited cycling life of rechargeable Zn-air batteries (ZABs) arising from the sluggish oxygen reduction/evolution reactions (ORR/OERs) severely hinder their commercial deployment. Herein, a zeolitic imidazolate framework (ZIF)-derived strategy associated with subsequent thermal fixing treatment is proposed to fabricate dual-atom CoFe─N─C nanorods (Co1 Fe1 ─N─C NRs) containing atomically dispersed bimetallic Co/Fe sites, which can promote the energy efficiency and cyclability of ZABs simultaneously by introducing the low-potential oxidation redox reactions. Compared to the mono-metallic nanorods, Co1 Fe1 ─N─C NRs exhibit remarkable ORR performance including a positive half-wave potential of 0.933 V versus reversible hydrogen electrode (RHE) in alkaline electrolyte. Surprisingly, after introducing the potassium iodide (KI) additive, the oxidation overpotential of Co1 Fe1 ─N─C NRs to reach 10 mA cm-2 can be significantly reduced by 395 mV compared to the conventional destructive OER. Theoretical calculations show that the markedly decreased overpotential of iodide oxidation can be ascribed to the synergistic effects of neighboring Co─Fe diatomic sites as the unique adsorption sites. Overall, aqueous ZABs assembled with Co1 Fe1 ─N─C NRs and KI as the air-cathode catalyst and electrolyte additive, respectively, can deliver a low charging voltage of 1.76 V and ultralong cycling stability of over 230 h with a high energy efficiency of ≈68%.

Low-Potential Iodide Oxidation Enables Dual-Atom CoFe─N─C Catalysts for Ultra-Stable and High-Energy-Efficiency Zn-Air Batteries.

Abstract Artificial photosynthesis using carbon nitride (g-C 3 N 4 ) holds a great promise for sustainable and cost-effective H 2 O 2 production, but the high carrier recombination rate impedes its efficiency. To tackle this challenge, we propose an innovative method involving multispecies iodine mediators (I − /I 3 − ) intercalation through a pre-photo-oxidation process using potassium iodide (suspected deteriorated “KI”) within the g-C 3 N 4 framework. Moreover, we introduce an external electric field by incorporating cationic methyl viologen ions to establish an auxiliary electron transfer channel. Such a unique design drastically improves the separation of photo-generated carriers, achieving an impressive H 2 O 2 production rate of 46.40 mmol g −1 h −1 under visible light irradiation, surpassing the most visible-light H 2 O 2 -producing systems. Combining various advanced characterization techniques elucidates the inner photocatalytic mechanism, and the application potential of this photocatalytic system is validated with various simulation scenarios. This work presents a significative strategy for preparing and applying highly efficient g-C 3 N 4 -based catalysts in photochemical H 2 O 2 production. 

pdf/circumventing-bottlenecks-in-h2o2-photosynthesis-over-carbon-3gia084wjc.pdf

Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects

Flexible zinc-air batteries (FZABs) have experienced rapid development due to the advantages of high theoretical energy density, wearable and notable safety. Wide-temperature FZABs have been challenged by rapid dehydration of gel-polymer electrolytes (GPEs) at high temperatures and freezing at low temperatures, as well as increased growth of zinc dendrites. Therefore, some studies have focused on constructing wide-temperature working FZAB using high water retention electrolytes while inhibiting the production of zinc dendrites. In this review, we first systematically examine several evaluation indicators for GPEs. Then, the strategies for improving the wide-temperature performance of GPEs are summarized based on four common polymer monomers. Additionally, reasonable strategies for suppressing zinc dendrites are explored. Finally, the future development directions for GPEs in FZABs are proposed. We hope that this review will provide guidance for the construction of wide-temperature and dendrite-free FZABs. 

Research progress in wide-temperature flexible zinc-air batteries

The storage time of Zn-air batteries (ZABs) for practical implementation has been neglected long-lastingly. ZABs based on organic solvents promise long storage time but suffer from sluggish kinetics. Here, we report a longly storable ZAB with enhanced kinetics mediated by iodine-containing redox. In the charge process, the electrooxidation of Zn5(OH)8Cl2·H2O is accelerated by I3- chemical oxidation. In the discharge process, I- adsorbed on the electrocatalyst changes the energy level of oxygen reduction reaction (ORR). Benefitting from these advantages, the prepared ZAB shows remarkably improved round-trip efficiency (56.03% vs. 30.97% without the mediator), and long-term cycling time (>2600 h) in ambient air without replacing any components or applying any protective treatment to Zn anode and electrocatalyst. After resting for 30 days without any protection, it can still directly discharge continuously for 32.5 h and charge/discharge very stably for 2200 h (440 cycles), which is evidently superior to aqueous ZABs (only 0/0.25 h, and 50/25 h (10/5 cycles) by mild/alkaline electrolyte replenishment). This study provides a strategy to solve both storage and sluggish kinetics issues that have been plaguing ZABs for centuries, opening up a new avenue to the industrial application of ZABs.

I3-/I- Redox Reaction-mediated Organic Zinc-Air Batteries with Accelerated Kinetics and Long Shelf Lives.

An Electrochemically Paralleled Biomass Electrolyte Additive Facilitates the Integrated Modification of Multi-dimensional Zn Metal Batteries

Strong Metal-Support Interaction to Invert Hydrogen Evolution Overpotential of Cu Coating for High-Coulombic-Efficiency Stable Zn Anode in Aqueous Zn-Ion Batteries.

Multifunctional hydrogels are widely applied in flexible electronics, energy devices, and sensors due to their unique physical and chemical properties. However, most hydrogels, particularly multifunctional ones, often require complex and time-consuming synthesis processes. Herein, we report a quadruple-functional hydrogel with complete reconstructability (6 cycles, dry fragments), self-healability (100 cycles, wet fragments), ultraextension (retaining >150-fold biaxial extension after reconstruction or self-healing), and redox-activity, synthesized via a simple and rapid method. This approach introduces hydrophobic I3- (endogenously generated from I2 and I-) directly into the polymer solution to trigger the Hofmeister effect in situ, eliminating conventional steps such as cooling-induced shaping and prolonged immersion. Capacitive sensors and self-powered temperature/strain sensor systems by this hydrogel completely retain their original performance after being rebuilt and self-healing. This work demonstrates a facile and efficient strategy for synthesizing multifunctional hydrogels, paving the way for their practical and delicate applications.

In Situ Hofmeister Effect in Polymer Solution by Hydrophobic I3- for Multifunctional Hydrogel.

Shape‐Memory Electrochemical Energy Storage Devices

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